Process of treating hydrocarbon fluids



May 18, 1937i J. RRosE PROCESS 0F TREATING HYDROCARBON FLUID Filed Dec. .20,

PatentedfMay 1s, 1937 raocEss or 'wrme mmnocAnnoN UIDS James lt. Rose, Edgewortli, Pa., assigner of threefourthsto Michael L. Benedum and Joseph C. Trees, both of Pittsburgh, Pa.,

`Application December 20, 1935, serial No. 55,387v

(ci. coi-31)' 5Claims.

This invention relates to aprocess of treating fluids consisting principally of aliphatic hydrocarbons for the production of valuable products therefrom. A eld wherein my process is of par- ,5 ticular importance is theproduction of benzene from hydrocarbon fiuids,'including natural gas or methane.

In my Patent No. 1,339,225, I describe and claim a process for manufacturing a gaseous fuel containing gases of the CHi and CsHs series by subjecting methane or natural gas to the heat of an electric arc formed between carbon electrodes.`

'Ihe present process contemplates such improvements over the process described and claimed in c the aforesaid 'patent as will enable me to produce, for instance, substantially pure benzene in a particularly `economical and efficient manner.

I realize my process by the apparatus shown in the drawing hereof, wherein the'view shows in vertical section a furnace or reaction chamber equipped .forf the production of benzene from hydrocarbon fluids and, on a reduced scale, a' diagrammatic illustration of an apparatus for separating and absorbing a heavy hydrocarbon,-such as benzene, -whereby it may be recovered as a liquid. 4 -0 Describing the apparatus by reference characters, I denotes 'the outer metallic wall of the upper section of an electric furnace or reaction chamber, having therein a lining 2, preferably of vcarbon blocks. 'Ihis upper section is shown as rest,

ing on any suitable support, as the bams 3 and Il, with a lower extension 6 having at the bottom an oiitake-connection 6 for the removal' of carbon or other non-volatile or non-gaseous material. From the lower section 6 there extends an offtake 'I for the gaseous mixture produced -within the furnace, which gaseous mixture 'is conveyed to separators andrecovered as aliquid and from which it c an bev drawn off. The apparatus used for separating the carbon from the gases and for the purification of gases and the absorption of the'enzene as a liquid may be any well known form-of apparatus employed for this purpose, such as projecting through an opening in a plate I6 secured to the furnace wall I and from each of which plates a bracket arm I 1v extends outwardly, each bracket arm supporting at its outer end a sleeve I8 through which a' threaded rod I9 exten s, the said rods being each engaged by an automatic feeding device 20, such as is well known in the industry. These rods are connectedto the carb'ons I0 and II and are adapted to maintain constant the distance between the inner ends thereof. Suitable .insulation 2l is` inserted, between each plate I6 and the furnace wall.

The carbon electrode Ill .and its operating rod I9 are connected through a housing 22 having at 4 its outboard end a chamber 22 with the flexible section 23*3L of a gas supply pipe 23 having a valve 23D. The inboard or furnacefacing end of this chamber is extended at 22bto form a tapered split sleeve which may be brought into engagement with the outer end of the carbon electrode I0 by means of a nut 24 having a tapered extension wall .24 adapted to engage the tapered surface ldicated at 25.

of the sleeve. Insulating material may. be in-` serted between the sleeve and the carbon, as introde I0, the electrode 26 extending through insulation 21 and the horizontal arm 28 of a bracket, the arm 29 of which is provided with a sleeve` 30 through whichextends the feeding rod 3l for v'the carbon 26, the said rod being driven by the automatic feeding device indicated generally at 32. The carbon 26 is supplied with gas through a pipe 33 in the same manner as the carbon I0, delivering the gas into a chamber 34 at the'outboard end of the housing-36, which is connected to the carbon 26 by means of a split tapered extension 34 of the housing and by the nut 35, 35,

as the separating chambers 8, which may contain I activated alumina, and from which the liquid benzene can be drawn olf through a-pipe t'.

Projecting into the furnace from opposite-sides thereof is the hollow carbon electrode Ill'and the solid carbon electrode II, the former electrode being a positive electrode and the latterI electrode being a negative electrode. I2 and I3 denote the electrical conductors which are connected to the said electrodes respectively. 4Each electrode is` provided with water cooling means comprising an annular water. chamber Il surrounding the 36 denotes theV conductor for supplying electric current to the carbon electrode 26, the said electrode being a positive electrode. The electrode 26 is provided with cooling means similar to those l employed with the electrodes I0 and II and consisting of an annular circulating chamber 31 and electrode adjacent to the furnace wall, each of.

the said chambers being provided with a cooling water supply pipe I5. Each electrode is shown a water supply p pe 38.

Gas supplied through the pipe 23 enters the lower extension of the furnace, where the pIpe' is formed into a coil 23, preferably located adjacent to the furnace wall. The upper or delivery end of the coil extends through the furnace wall Aand to the casing of the valve 23h. 39 denotes any conventional high-frequency apparatus 55 applied to Ya suitable portion of the pipe I3 and al capable of subjecting the gas in this portion of the pipe to the disruptive action of the are, the saidl device being provided with vthe conductors 40 and 4I; .The high-frequency apparatus may 60 be one of the type manufactured by the General Electric Company and the Westinghouse Electric & Mfg. Company, comprising a chamber through which the gas is conveyed, said chamber containing non-sparking high-frequency coils, whereby an initialdissociation of the gas i's instituted, which dissociation is completed by the arc formed between-the electrodes. Frequencies of 12,000,000 cycles per second are conventional and may be employed herein. Belowthe electrodes, shelves 42 project into the furnace from the lining, said shelves containing a catalyst 43, such as platinum black, finely divided nickel, or iron ore, which will increase the yield of benzene.

With the parts constructed and arranged as described, my process will be carried outas follows-Hydrocarbon fluid will be supplied through the pipe 23 to the bottom of the coil 23C, whereby the fluid is raised to such a temperature as to materially reduce the electric current re' quired for its dissociation within the furnace. In its passage from the Vcoil to the electrode l0, it is subjected to the disruptive action of the high frequency current whereby a partial dissociation of the fluid is produced. When delivered into the interior of the arc formed between the electrodes I0 and Il or into the region of the arc, further dissociation takes place. When the hydrocarbon uid is methane or natural gas, it is dissociated in accordance with the reaction (KCI-I4) =C6H6|18H.

Notwithstanding the fact that this reaction indicates the liberation of an excess of hydrogen, it has been found that additional hydrogen is necessary in order to insure the production of benzene and also to prevent the destruction of the carbon lining of the furnace. In other words, by introducing hydrogen through the carbon 26 into the region of the arc, hydrogen is always available in sufficient quantity and proportion to insure the production of the benzene and also to prevent or limit the liberation of carbon in excess of that required to produce the benzene. By introducing the hydrocarbon uid into the interior of the arc between the electrodes I0 and H 'and delivering the hydrogen into the region surrounding the said arc, the fluid is subjected to the action of the arc for an appreciable interval of time before coming into contact with the hydrogen. It is my belief that it is due to the conjoint action of the heat of the arc supplemented by the hydrogen introduced through the electrode 26 that I am enabled to produce from hydrocarbon uid benzene in such quantities as to render its recoverycommercially successful.

The benzene in gaseous form, together with the surplus hydrogen and whatever small proportion of carbon black may have been produced. is delivered through the furnace extension 5, and the gaseous products are delivered thence by the offtake 1 to the separator and absorber shown at 8, 8.

Whatevervcarbon black may be formed in the practice of my process can be drawn on at the bottom of the furnace, as indicated at 6, and may be Vconducted through such conventional carbon separators additional thereto` as may be desirable or necessary for the recovery of the In place o1' using hydrogen from a separate source of hydrogen supply for the electrode 26, I may employ for this purpose such proportion as may be necessary o'i' the excess gas yliberated in the practice of my process. In this event, the gas, which consists essentially of hydrogen, will be conveyed from the separating and absorbing apparatus indicated at 8, 8 through the pipe 44, said pipe having therein a three-way valve 45 by means of which as much of the gas may be directed to the electrode as may be desired, the remainder of the gas being delivered elsewhere through the pipe 46.

'I'he separating and absorbing apparatus 8, 8,

' as stated hereinbefore, may be of any standard arc; and immediately thereafter contacting the products resulting from the action of they arc with a polymerization catalyst immediately adjacent to said arc. .4

2. The herein described process of manufacturing benzene which comprises supplying a gas consisting principally of methane continuously through and beyond the arc produced between electrodes in a reaction chambencontacting the resultant gaseous mixture immediately thereafter with a solid polymerization catalyst, with no substantial reduction of the temperature of said mixture, removing carbon and recovering benzene in liquid form from the gases thus produced and de-carbonated, and delivering gaseous products resulting from such separation into the arc, in subsequent cycles of operation.

3. In the process claimed in claim 2, preheatl ing the gas which consistsI principally of methane and subjecting it to the action of the disruptive discharge of a high frequency Vcurrent prior to its circulation through and beyond the arc formed between the electrodes in the reaction chamber.

4. The herein described process of producing benzene which comprises supplying a hydrocarbon uid consisting principally of aliphatic hydrocarbons continuously through an arc produced between electrodes in a reaction chamber thereby to dissociatesaid fluid; and immediately thereafter contacting the products resulting from the action of the arc with a. solid polymerization catalyst immediately adjacent to said arc and with no substantial reduction of the temperature of said mixture. A

5. The herein described process of producing benzene which comprises supplying a hydrocarbon iluid consisting principally of aliphatic hydrocarbons continuously through an arc produced between electrodes in a reaction chamber thereby to dissociate said duid, immediately thereafter contacting the products resulting from the action of the 'arc with asolid polymerization catalyst immediatelyl adjacent to said arc and with no substantial reduction of the temperature of said mixture, and delivering hydrogen into the arc together with the aforesaid hydrocarbon iuid.

f JAMES R. ROSE. y 

